The collection consists of fifty-five Greek manuscripts acquired by the Library since its founding in 1610, including those received from Sion College in 2006. The MSS date from the tenth to the nineteenth centuries and include:

Gospel Books and Lectionaries, Acts and Epistles Books and Lectionaries, and the Book of Revelation

Octateuch with catena (MS 1214)

Patristic and other theological texts including works of John Chrysostom (Sion L40.2/G5), Gregory of Nazianzus (Sion L40.2/G7), and John of Damascus

Post-Byzantine texts including a Chronicle in vernacular Greek by an anonymous author (MS 1199), and Damaskenos Stoudites, On Animals (Sion L40.2/G12).

Among the most important manuscripts is MS 461, containing a theological treatise on the procession of the Holy Spirit by George Scholarios (later Ecumenical Patriarch of Constantinople Gennadios II), with his autograph signature, notes and corrections. This was left to the Library by Archbishop Abbot (d.1633).

Many of the manuscripts (MSS 1175-1207) were collected during his visits to the eastern Mediterranean by J.D. Carlyle, Professor of Arabic at Cambridge, for a proposed new critical edition of the New Testament which was left unfinished on his death in 1804, though collations by Carlyle’s assistants can be found in MS 1255. Some of the Carlyle manuscripts were returned to their rightful owner, the Patriarch of Jerusalem, following their acquisition from Carlyle's heir by Archbishop Manners-Sutton in 1806. The work of collation was carried on by Charles Burney who left the fruits of his examination of the Carlyle MSS to the Library on his death in 1817 (MSS 1223-1224, 1259).

Further information can be found in: Todd, H.J. An account of Greek manuscripts, chiefly biblical which had been in the possession of the late Professor Carlyle ... now deposited in the archiepiscopal library at Lambeth Palace, [1823].

The Greek Manuscript Collection of Lambeth Palace Library, An exhibition held on the occasion of the 21st International Byzantine Congress, London, 22-23 August 2006 (London, 2006).